Impact of vibrational modes in the plasmonic purcell effect of organic molecules
EntityUAM. Departamento de Física Teórica de la Materia Condensada
PublisherAmerican Chemical Society
10.1021/acsphotonics.0c01095ACS Photonics 7.12 (2020): 3369–3375
Funded byThis work has been funded by the National Natural Science Foundation of China under Grant No. 11804283, by the European Research Council through Grant ERC-2016-STG- 714870, and by the Spanish Ministry for Science and Innovation − AEI Grants RTI2018-099737-B-I00, PCI2018- 093145 (through the QuantERA program of the European Commission), and CEX2018-000805-M (through the “Maria de Maeztu” Programme for Units of Excellence in R&D). A.I.F.-D. acknowledges support from a 2019 Leonardo Grant for Researchers and Cultural Creators, BBVA Foundation. D.Z. acknowledges financial support from the China Scholarship Council to fund his stay at Universidad Autónoma de Madrid as a postdoctoral fellow
Projectinfo:eu-repo/grantAgreement/EC/H2020/714870/EU//MMUSCLES; Gobierno de España. RTI2018-099737-B-I00; Gobierno de España. PCI2018-093145; Gobierno de España. CEX2018-000805-M
Subjectsemission spectrum; excited-state dynamics; Fermi's golden rule; single vibrational mode model; tensor networks; two-level system; Física
Rights© 2020 American Chemical Society
Esta obra está bajo una licencia de Creative Commons Reconocimiento-NoComercial-SinObraDerivada 4.0 Internacional.
By means of quantum tensor network calculations, we investigate the large Purcell effect experienced by an organic molecule placed in the vicinity of a plasmonic nanostructure. In particular, we consider a donor-πbridge-acceptor dye at the gap of two Ag nanospheres. Our theoretical approach allows for a realistic description of the continua of both molecular vibrations and optical nanocavity modes. We analyze both the ultrafast exciton dynamics in the large Purcell enhancement regime and the corresponding emission spectrum, showing that these magnitudes are not accurately represented by the simplified models used up to date. Specifically, both the two-level system model and the single vibrational mode model can only reproduce the dynamics over short time scales, whereas the Fermi's golden rule approach accounts only for the behavior at very long times. We demonstrate that including the whole set of vibrational modes is necessary to capture most of the dynamics and the corresponding spectrum. Moreover, by disentangling the coupling of the molecule to radiative and nonradiative plasmonic modes, we also shed light into the quenching phenomenology taking place in the system
Google Scholar:Zhao, Dongxing - Silva, Rui E.F. - Climent, Clàudia - Feist, Johannes - Fernández Domínguez, Antonio Isaac - García-Vidal, Francisco J.
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